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Electrical control of magnetism has great potential for low-power spintronicsapplications and the newly discovered two-dimensional van-der-Waals magneticmaterials are promising systems for this type of applications. In fact, it hasbeen recently shown experimentally that upon electrostatic doping by electronsbilayer CrI3 undergoes an antiferromagnetic-ferromagnetic (AFM-FM) phasetransition, even in the absence of magnetic field. Doping by holes, on theother hand, does not induce the same transition in the experiment, which pointsto an intrinsic asymmetry in the hole and electron doping that limits thecontrol of the transition by doping. We here show, based on first-principlescalculations, that the asymmetry originates in the relativistic nature of thevalence-band-edge states of the pristine bilayer, which inhibits the magnetictransition upon hole doping. Based on this finding, we propose an approach toengineer this system so that it displays the AFM-FM transition for both holeand electron doping by using moderate uniaxial strain along the soft directionof the bilayer.

Overcoming the asymmetry of the electron and hole doping for magnetic transitions in bilayer CrI3